Food compositions incorporating cellulose crystallite aggregates



United States Patent 3 (923 we soon coanosrrroNs nconroaarmo CELLU- LOSECRYSTALLITE AGGREGATES Orlando A. Battista, Drexel Hill, Pa, as'signorto American Viscose Corporation, Philadelphia, Pa., 2 corporation ofDelaware No Drawing. Filed July 5, 1960, Ser. No. 40,517

8 Claims. (Cl. 991) This invention relates to reduced calorie foodcompositions comprising a food material and, as a nonnutritive agent,cellulose crystallite aggregates, the latter comprising a product of theacid hydrolysis of cellulose. More particularly, the invention relatesto reduced calorie food compositions having an eating quality at leastequal to that of the food material per se and in many cases improvedthereover.

Interest in low calorie foods is today very large and is steadilyincreasing. The demand for such foods in the US. comes from a groupwhich, according to a 1957 surve, is estimated as one-half to two-thirdsof the population, and which includes the overweight, the pregnant, thediabetic, etc. According to a 1959 report, there are thirty-four millionAmericans in the over- Weight class alone; and the same source revealsthat at least a quarter billion dollars is spent annually on low caloriefoods. It has been pointed out more recently that an increasingproportion of the US. juvenile population is becoming fat and is in needof being made calorie conscious.

The need is a long standing one, and efforts have been and are beingmade to satisfy it. Leaving aside the non-prescription reducing pillsand gadgets, for which large sums are spent, many of the reduced caloriefoods heretofore developed have poor flavors, which reflects the factthat no satisfactory bulking material is available to manufacturers ofthese foods. Many of such foods have been reduced in calories bysubstituting artificial sweeteners for sucrose, or by reducing fatcontent. At present, saccharine, cyclamates, methyl and carboxymethylcellulose, and sea weed derivatives are the main non-nutritive materialsadded to foods, and in each case these products are added at very lowlevels, since the limiting factor of undesirable flavors is inherent ineach of them. Conventional fibrous cellulose has been used as a bulkingagent, but the great defect of this material is-its objectionabletexture; thus, when mixed with a food or food ingredient and the mixturetasted, it is noticeable per se to the taste, is not smooth, has afibrous mouth feel when chewed, gives the impression of thepresence ofan additional insoluble or residual substance, and tends to accumulatein the mouth. The unsatisfactory texture of the fibrous materialcannotbe remedied no matter how small the fibers are cut. Soluble cellulosederivatives have also been used as bulking agents but tend to formunpalatablegummy masses in the mouth.

To help meet the present and potential demand for low calorie foods, theinvention provides food compositions that will satisfy the appetite ofthe consumer, enable him to continue to enjoy eating, and yet avoid thehealth problem arising from over-consumption of calories. These dieteticcompositions incorporate cellulose crystallite aggregates, which asindicated, are a product of the acid hydrolysis of cellulose, and aredescribed below in detail. The aggregates per se, it may be recorded,are bland in taste and odor, white in color, have a physical appearanceresembling starch, and are edible but not nutritious. They are entirelyfree of the objectionable textural defects of agents like conventionalfibrous cellulose, which adversely change the taste and mouth feel ofthe food with which they are mixed; rather, the aggregates areparticularly characterized by 3,023,104 Patented Feb. 27, 19 62 2 havinga smooth pleasant mouth feel, by becoming an indistinguishable part ofthe food with which they are mixed, and by simulating its eatingquality.

It will be understood, therefore, that the cellulose crystalliteaggregates help to provide low calorie food products while yet enablingthe products to meet recognized standards of acceptability, particularlyin respect of the essential property of mouth feel or eating quality. Inother words, the aggregates afford a reduction in calorie content withno sacrifice of the familiar qualities of time-tested foods. eyond this,and coincidently, therewith, the aggregates are capable of improvingmany foods, and the processing thereof, in a number of other respects.Thus, they permit desirable variations to be made in the physicalcharacteristics of a food, such as its eating quality, appearance,cohesiveness, and texture, including its tactual, visual, and tastetextures. For example, liquids and pastes may be formed into a crumb,and oily materials into a plastic mass like butter. A- desirableproperty may be given to a food whichlacks' it, thus thickness may beimparted to a salad dressing; Or a less desirable characteristic of afood may be reduced, as in the case of candy of pronounced sweetness,where the presence of the aggregates tends to lessen the sweet taste. Inother cases, improvementsxand advan= tages are realized in theprocessing of the'food ma terial, as by increasing the yield, orsimplifying the handling of oily or sticky materials.

The invention, in brief, comprises a reduced calorie food compositioncomprising a food material and cellu lose crystallite aggregates havinga level-elf D.P.. (.degree of polymerization). i

This application is a continuation-in-part of applicants copendingpatent application Serial No. 836,320; filed August 27,1959. q

As indicated, the cellulose crystallite aggregates are" productsobtained by. the controlled acid hydrolysis of cellulose, there beingformed an acid-soluble portion and an acid-insoluble portion. The lattercomprises a crys-' talline residue or remainder which is washedcandrecovered, being referred to. as cellulose-crystallite aggregates, or aslevel-0d D.P. cellulose.

In the acid hydrolysis, the acid. dissolves amorphous portions of theoriginal cellulose chains, the undissolved portions being in aparticulate, non-fibrous or crystalline: form as a result of thedisruption of the continuity of the fine structures between crystallineand amorphous regions of the original cellulose. Although hydrolysis,

may be effected by various specific methods, including the use ofvarious acids, a direct method which is" free" of secondary reactionscomprises the treatment of the original cellulosic material with 2.5normal hydrochloric acid solution for 15 minutes at boiling temperature.Another suitablemethod comprises treating the ce1lu'-' losic materialwith 0.5% hydrochloric acid solution (0.14 normal) at 250 F. for 1 hour.The'cellulose under going such treatment reaches, within the timeperiodnoted, a substantially constant molecular weight, or, in otherwords, the number of repeating units or monomers,

sometimes designated anhydroglu-cose units, which make" up thecellulosic material, becomes relatively constant, from which it isapparent that. the degree of polymerization of the material has leveledoff, hence the name levelolf DP. cellulose. In other words, if thehydrolysisreaction were continued beyond the period noted, the DP. wouldchange very little if at all. In all cases, the level-cit D.P. valuereflects the fact that destruction of the fibrous structure has occurredas a result of the substantially complete removal of the amorphousregions of the original cellulose.

It may be observed that crystal-lite, as used herein, is a cluster oflongitudinally disposed, closely packed cellu 3 lose chains ormolecules, and that aggregates are clusters of crystallites. Theaggregates may also be said to comprise straight rigid, relativelynon-twistable groups of linear chains. As indicated by X-ray diffractiontests, the crystallites and crystallite aggregates have a sharpdiffraction pattern indicative of a substantially crystalline structure.Although the crystallite chains are of very uniform lengths,particularly by comparison with the original cellulose chains, strictlyspeaking they do exhibit some variation, and for this reason it ispreferred to speak of average length, or of average level-E D.P. values.

The hydrolysis methods noted above are particularly characterized inthat in each crystallite aggregate resulting from the hydrolysis, noconstituent chain is connected to a chain in a neighboring aggregate;rather all the chains in an aggregate are separate from and free ofthose in neighboring aggregates.

The cellulose crystallite aggregates, or level-off D.P. cellulose,suitable for use in the invention is characterized by having a preferredaverage level-cit D.P. of 125 to 375 anhydroglucose units. Ideally,within this range all of the material should have the same D.P., orchain length, but as this is difiicult if not impossible to achieve, itis preferred that at least 85% of the material have an actual D.P. notless than 50 and not more than 550. More preferably, at least 90% of thematerial should have an actual D.P. within the range of 75 to 500, andit is still more preferred if at least 95% of the material has an actualD.P. in the range of 75 to 450. It may thus be apparent that the chainlength of the level-off D.P. cellulose, or cellulose crystalliteaggregates, is very uniform, a consequence of the hydrolysis, whereinthe longer chains of the original cellulose were converted to shorterchains and the very short chains were dissolved away. In short, thehydrolysis effected a homogenization of the chain length distribution.As may also be apparent, a reference to crystallite aggregates having anaverage level-off D.P. of 125 means that the aggregates have an averagechain length corresponding to 125 anhydroglucose units, and inaccordance wtih the first preference noted above, at least 85% of thismaterial will be made up of chains containing 50 to 350 such units; theremaining may comprise shorter and/or longer chains.

More preferably, the average level-ofi D.P. is in the range of 200 to300, .of. which material at least 90% has an actual D.P. in the range of75 to 550.

Associated with the foregoing D.P. properties of the crystalliteaggregates is the fact that their chemical purity is very high, thematerial comprising at least 95 preferably at least 97% or 99%,polyglucose, or anhydroglucose units, based on chromatographic analysis.In terms of ash content, the aggregates preferably contain less than 100p.p.m. (parts per million), although ash may range from about 10 toabout 400 or 500 or 600 p.p.m. By comparison, conventional fibrouscellulose may have 1000 to 4000 p.p.m. of ash. In connection with thepurity of the aggregates, it may be explained that the inorganiccontaminants in the original cellulose, which are concentrated in theamorphous regions. thereof, are dissolved away by the hydrolyzing acid,and the non-cellulose components of the original material are soeffectively destroyed that their concentration is reduced to a very lowlevel. Of interest is the fact that the chains produced by thehydrolysis each have on one end thereof a potential aldehyde group, suchgroup being in the 1 carbon position of an end anhydroglucose unit andrequiring the assistance of the ring oxygen atom, whch is ortho to it,to realize its aldehydic potential. The group has the reducing properties of an aldehyde group. On their other ends the chains have onlyhydroxyls as functional. groups.

The aggregates resulting from the hydrolysis and washing steps arefurther characterized by having a particle size in the range of 1 or 2to 250 to 300 microns, as determined visibly by microscopic examination.By subfooting the foregoing product to a mechanical disintegration, asdescribed below, there is produced a material having a size in the rangeof less than 1 to about 250 or 300 microns. Within this range, theparticle size and size distribution are variable, it being understoodthat the size and size distribution will be selected to suit aparticular end use. In general, mechanically disintegrated particles arepreferred.

The source material for the crystallite aggregates may suitably be oneor more natural fibers such as ramie, cotton, purified cotton, alsobleached sulfite pulp, bleached sulfate wood pulp, etc. Particularlysuitable are sulfite pulp which has an average level-ofl D.P. of 200 to300, at least 90% of which has a D.P. in the range of to 550; and alsosulfate pulp which has an average level-off D.P. of 125 to 175, at leastof which is in the range of 50 to 350.

Other suitable cellulose crystallite aggregates may have lower averagelevel-ofi D.P. values, say in the range of 60 to 125, or even 15 to 60.Aggregates from both of these ranges have the chemical purity and othercharacteristics of the aggregates from the first noted D.P. range.Crystallite aggregates in the 60 to 125 average level-off D.P. range areobtainable from the acid hydrolysis of alkali-swollen natural forms ofcellulose, of which a preferred source is cellulose that has beenmercerized by treatment with 18% caustic soda solution at 20 C. for twohours. Aggregates in the 15 to 60 average leveloti D.P. range aresuitably prepared from regenerated forms of cellulose, including tireand textile yarns, other regenerated cellulose fibers, and cellophane.

In general, the cellulosic source material has a D.P. greater than thelevel-off D.P. thereof.

As obtained from the acid hydrolysis and water washing steps, theaggregates in the over-all average level-ofl D.P. range of 15 to 375 arein a loosely aggregated state, particularly in the larger sizes, sayfrom 40 to 250 or 300 microns, and are characterized by the presence ofmany cracks in their surfaces, including similar surface irregularitiesor phenomena like pores, depressions, voids, fissures and notches.Because of such irregularities, the apparent or bulk density of theaggregates is much less than their absolute density. Furthermore, thecracks and other irregularities persist despite the application of highcompressive forces on the aggregates. Thus, when they are compressed at5,000 p.s.i., they exhibit an apparent density of 1.26; at 10,000 p.s.i.the apparent density rises to 1.32; at 15,000 p.s.i. it is 1.34; and at25,000 and 37,000 p.s.i. it is 1.38 and 1.38 respectively. On the otherhand, the absolute density of a unit crystal or crystallite is 1.55 to1.57, from which it is apparent that the aggregates occlude considerablequantities of air in the surface cracks, voids, fissures, etc. Theapparent densities of the dried disintegrated aggregates, at thecompressive forces noted, are somewhat higher than the foregoing values.Of interest in this connection is the fact that the aggregates, dried ornever dried, retain their pressed form after compression; in otherwords, three-dimensional structures of any desired shape may be formedby compressing the aggregate particles.

Either before or after mechanical disintegration the aggregates may bedried. Where the disintegration is performed in the presence of anaqueous medium, drying is preferably carried out after thedisintegration step. Drying may be done in any suitable vacuum, or inair at room temperature or higher, going up preferably to 60 C. to 80C., although the temperature may be up to or C. or higher. Anotherprocedure is to displace the water in the wet aggregates, preferably bymeans of a low boiling, water miscible organic compound such as a lowmolecular weight aliphatic alcohol like methanol, ethanol, propanol,isopropanol, etc., and then to evaporate off the compound. The resultingdried aggregates tend to be more reactive and, as described below, toform stable dispersions and gels more readily. Spray drying either inair or in a vacuum is also satisfactory. Spray drying, and also freezedrying and drum drying, are particularly effective to dry the aggregatesafter the disintegration step. Freeze drying in particular favors thedevelopment of a very porous, reactive material which is characterizedby the presence therein of a multiplicity of pores or depressions ofextremely small size; such material readily forms stable dispersions andgels.

Mechanical disintegration of the aggregates, as referred to above, maybe carried out in several ways, as by subjecting them to attrition in amill, or to a high speed cutting action, or to the action of highpressures on the order of at least 5,000 or 10,000 psi. The invention ofdisintegration by pressure is the invention of Orlando A. Battista andPatricia A. Smith and is disclosed in the copending application SerialNo. 27,268, filed May 6, 1960. The disintegration of the aggregates iscarried out in the presence of a liquid medium, although where highpressure alone is employed, such medium, although desirable, is notnecessary. Water is a preferred medium, but other preferably edibleliquids are suitable, including sugar solutions, polyols, of whichglycerol is an example, alcohols, particularly ethanol, and the like.Whatever method is used, the disintegration is carried out to such anextent that the resulting disintegrated aggregates are characterized byforming a stable suspension in the aqueous medium in which they arebeing attrited, or in which they may be subsequently dispersed. By astable suspension is meant one from which the aggregates will not settleout but will remain suspended indefinitely, even for periods measured interms of weeks or months. The disintegrated aggregates are furthercharacterized by the fact that such suspension forms an extremelyadherent film when deposited on a glass panel or sheet or other suitablesurface. At lower concentrations of aggregates, the suspension is adispersion, while at higher concentrations it is a gel.

The preferred disintegration method is to attrite the aggregates bymeans of a high speed cutting action in the presence of an aqueousmedium. The aggregates may be in a dry or never-dried state prior toattrition, although some water should be present during the cutting orshearing of the particles. If they are initially in the neverdried orwet state, that is, as received from the water washing step, they have amoisture content of at least 40% by weight, and it is possible toattrite them without further addition of Water, although water may beadded if desired. In any event, its preferred that the water content ofthe mixture undergoing attrition should be at least to to by weight. Theaggregates content of the mixture to be attrited is preferably at least3% by weight, and desirably is higher as the efliciency of the cuttingaction increases with the aggregates content.

Suitable consistencies are those of mixtures containing up to about byweight of aggregates and the balance water; such mixtures lendthemselves well to good attrition and are convenient to handle bothduring and after the disintegration; they also have the advantage ofdirectly producing a gel. At consistencies above 35%, say from 35 to70%, attrition produces a material which, in the lower end of thisrange, resembles mashed potatoes of relatively soft or mushy appearance,and as the concentration increases, the material acquires aprogressively firmer and drier appearance and consistency; above thematerial tends to become crumbly. Although the attrited products ofconsistencies above 35% are not gels, t ley have the distinctiveproperty of forming indefinitely stable, smooth gels of varyingthickness and striking appearance upon the addition of water andstirring manually, as with a spoon, for a few minutes. At about 80%consistency, attrition results in a damp but free flowing materialcomprising discrete grains or granules and clumps of grains; themoisture content is apparent to the touch rather than the eye; and thematerial forms a gel upon being manually stirred or beaten in water. At80 to 90% consistency, the product of attrition is a crumbly, freeflowing, grainy, dry-appearing material that does not have a damp feeland which requires energetic beating in the presence of water to form agel.

It may be useful to review briefly the characteristics of thedispersions and gels. They comprise attrited products of an attritablemixture having a solids content of at least 3% by weight during theattrition step. Necessarily, the resulting attrited product will alsohave at least 3% solids, although, as indicated, some useful materialsare obtainable by diluting such attrited product to a consistency of 2%solids, or even 1%, to form a stable dispersion. In the next place, atleast 1% by weight of solids in the product of attrition have a particlesize of up to 1 micron. In the third place, the attrited product, indispersion or gel form, forms substatiallyadherent films, preferablysubstantially continuous and self-supporting films, when applied to asuitable surface. Finally, the attrited product is, or forms, a stableand homogen eons colloidal dispersion or gel, the term homogeneousreferring to the uniform visual appearance of the dis persion or gel.With respect to the last mentioned characteristic, it will beunderstood, as described, that attrited products having more than about35% solids, al though not gels, will easily form a gel upon manualstirring in water. It should also be understood that stable,

' homogeneous, colloidal dispersions and gels, as contemplated herein,are free of layers or sediment; there is no bottom layer of sediment;nor is there a top layer of visibly lower solids content than thebalance of the mixture. Rather, the stable dispersions and gels areuniform and homogeneous throughout; have a uniformly white color, somemixtures being more, or less, intensely White than others, depending onthe aggregates content and particle size distribution; and are furthercharacterized by having a very smooth butterlike mouth feel. Thepreferred dispersions and gels are those that are stable for at least amonth, and another preferred group comprises those stable for at least aweek. Dispersions and gels that are stable for at least a day, or evenan'hour, are also useful for some purposes, as where they are to be usedalmost immediately. But as may be apparent, the more stable dispersionsand gels have the advantage of being storable for a considerable periodof time.

Generally, the concentration of aggregates in' the aqueous dispersionsis at least 3% by weight,v and more preferably at least 4 or 5%. It ispossible to make stable homogeneous dispersions having a solids contentof up to 6 to 8% by weight, although more usually the solids rangs from3 to 6%. In the case of gels, the aggregates content varies from 3 or 4%to about 30 or 35% by weight, the upper concentration being limited onlyby the capacity of the gel to be handled or Worked. The concentrationboth of dispersions and gels may be varied-not only by varying theconsistency of the attritable mixture but also by adding water to thedispersion or gel, and, less preferably, by evaporating water therefrom.Usually the gels are thixotropic when they contain about 8 to 10% byweight, or more, of the aggregates. As may be apparent, the moreconcentrated dispersions may have a solids content which overlaps thatof the less concentrated gels. The fact that gels are obtainable atconcentrations as low as 3 or 4% solids is explainable by the presenceof considerable amounts of aggregates of a particle size ofsubstantially 1 micron and less, it having been found that gel formationis favored as the concentration of these fine particles increases. Infact, at concentrations as low as about 3% solids, gels are obtainablewhich are thixotropic provided the aggregates are substantially all of 1micron size and less.

Following the mechanical disintegration of the aggregates, the resultingproduct, whether a dispersion or gel, may be taken and used as such; orit may be de-watered and dried; or it may be desirable to fractionate itinto fractions having a more uniform particle size and sizedistribution. If the product is a mixture containing 35 to 90% solids,it may be stirred in water to form a gel, and the latter is handled asindicated. The dried products are also redispersible in aqueous media bythe help of agitation, such as provided by a Waring Blendor, to formdispersions and gels.

In respect of the drying of the gels, it should be observed, first ofall, that the preferred gels are thos obtained by attriting thenever-dried hydrolysis product; these gels have very desirable qualitiesin respect of smoothness, mouth feel, firmness, storage characteristics,etc. They may be dried to any practical moisture content, in which statethey are redispersible in water, by the aid of a suitable attritionstep, to form a gel, and this latter gel may again be dried if desiredand again redispersed to form a subsequent gel. Gels are also obtainableby attriting the dried hydrolysis product, and these gels may be driedand attrited to again form gels. For producing the dried products, anumber of drying procedures are available, and while redispersiblematerials result from each procedure, some procedures are moreadvantageous than others, as indicated. For example, freeze drying,spray drying, drum drying, and drying by solvent displacement eachproduce a material which has an appreciably lower bulk density thanconventionally oven-dried materials, with freeze drying producing thelowest bulk density by far, vis., 9.8 lbs/cu. ft. as against 14.1lbs/cu. ft. for oven-dried aggregates; each such procedure produces amaterial which is more easily redispersible in water, by the aid of anattrition step, to form a stable suspension than air or oven-driedmaterials; and each said procedure yields a more reactive product thanair-dried or oven-dried products. Freeze-dried, spraydried, drum dried,and solvent displacement-dried materials arc noticeably softer to thetouch than products of the other drying steps; and freeze drying alsoproduces a more porous product. With regard to the mouth feel of thevarious materials, those made by freeze drying, spray drying, and drumdrying, are superior.

Fractionation of the attrited products may be accomplished by means ofsuch separation procedures as mechanical sifting, settling in Water, orcentrifuging, a number of useful fractions being obtainable, includingfractions having a particle size of up to 0.2, 1, 2, 5, or 10 microns.Still another desirable fraction is one whose dimensions are all below100 microns, or below 40 or 50 microns; a fraction in the range of about40 to 250 or 300 microns is of special interest because of the findingthat particles in this size range, particularly those having one or twodimensions of up to 250 or 300 microns, tend to have cracks, fissures,notches, voids, depressions, pores, and the like in their surfaces.Preferably, each dimension of the particles should be within the sizerange noted for each fraction; however, particles having two dimensionswithin the size range are quite useful, as are particles having but onedimension within the size range although they are less preferred.

It will be understood that either dispersions, or gels, or fractionsthereof, or attrited mixtures dilutable to a dispersion or gel, may beemployed for preparing a food composition. Preferably, a gel is used.

The invention is broadly applicable to any food, food composition, foodingredient, or food product, whether comprised of a single ingredient ora mixture of two or more ingredients, whether liquid, liquid-containing,or solid, whether mainly carbohydrate, fat, protein, or any mixturethereof, whether edible per se or requiring preliminary conventionalsteps like cooking, mixing, cooling, mechanical treatment, and the like.

The invention is particularly applicable to bakery products, includingthe several varieties of bread, cake, cookies, crackers, biscuits, pies,and doughnuts; snack items like pretzels and potato chips; otherpastries and specialties; also prepared mixes for making any of theforegoing products; and in cereals, flours, and macaroni products. Bakedgoods mainly comprise starch, and this containing meat mixtures.

is particularly true of cookies and crackers. The starch content is sopredominant that heretofore it has been very dih'icult, if not out ofthe question, to reduce the calorie value of these products to anyappreciable extent without impairing their taste; but by virtue of thebland quality of the crystallite aggregates and their smooth mouth feel,it is possible to reduce substantially the calorie value of many bakedproducts without restricting their appeal. In other words, theaggregates may replace considerable amounts of flour in the foregoingproducts. They may also replace, in whole or part, bread additives likedextrins and starch. In the case of products made of finely groundflour, such as cakes and cookies, the aggregates serve to retainmoisture and other liquids, and, in effect to increase theliquid-carrying ca pacity of such flours, thus helping to avoid stalingof the products for longer periods of time, a result of particularadvantage for high sugar-containing cakes. The use of the aggregatesalso enables normally liquid ingredients to be handled in asubstantially dry free-flowing form; that is, the liquid ingredients mayfirst be mixed with the aggregates to form a substantially dry granularmixture and the latter can then be added to the recipe mix. In effect,the liquids are dried, although actually they are sorbed, that is, bothadsorbed and absorbed, by the aggregates. Such liquid ingredients mayinclude shortening materials, water, milk, syrups, and emulsifiers; andother suitable ingredients are lard, butter, and eggs.

7 The crystallite aggregates have utility in foods comprisingprincipally carbohydrates, such as sugars and starches, being capable ofdirect incorporation therewith and of being used wherever such foods areused, as in puddings, custards, and toppings, and in dry mixes forpreparing the same. In the case of dry mixes, the aggregates are notonly useful for making up the mix but also they help retain aqueous andoily ingredients therein, i.e., they prevent leaching out of the liquidas by surption onto the walls of the package in which the dry mixes aredistributed and sold.

The invention is of value in foods like dressings and spreads which areprepared by the aid of edible fats and oils, including shorteningagents, butter, margarine, cooking and salad oils, plastic fats, lard,etc. Besides reducing the calorie value of the product and assisting tohold the ingredients together, particularly the liquids, the aggregatesprovide a desirable thickening effect.

The preparation of meat and meat products, including sausage, sausageproducts, meat loaves, etc. comprises another appropriate area for theutilization of the crystallite aggregates. In the manufacture of sausageproducts and meat loaves the aggregates help to simplify the processingsteps by making the meat emulsions and meat mixes easier to handle, anadvantage brought about by the sorptive capacity of the aggregates forthe liquid- The consistency and stability of a meat emulsion, forexample, may be regulated in this way, and thus the cohesiveness of thefinal product may be varied. Coincident with the drying or sorptioneffect is the improved retention of flavors, water, and fats. As aconsequence of fat and water retention, there will be less free fat inthe product, and less shrinkage. Texture, juiciness, and otherorganoleptic characteristics may be improved by varying the firmness,juiciness, chewiness, etc. of a sausage or meat loaf product.Convcntional binders like cereals, starches, and flours, which are allnutritious, may be replaced in whole or part by the crystalliteaggregates, as may other frequently used meat loaf ingredients likemacaroni, cheese, potatoes, etc. Better distribution of seasoningmaterials may be secured by first mixing them with the aggregates andthen adding the mixture to the meat emulsions or mixes. The crystalliteaggregates favor the formation of paste and paste-like products sincethe aggregates are quite amenable to being spread, especially in thepresence of The aggregates may replace, at least partly, the

liquids.

use of ice to obtain a proper consistency and stability in meatemulsions; thus the aggregates may make it possible to achieve adesirable consistency by the use of water at room temperature and soavoid the necessity of refrigeration. An advantage of economicimportance is the increased yield of the meat emulsion or meatmix'obtainable when the aggregates are employed.

In one instance, hamburgers were prepared containing 5, 10, 15, and 20%of the aggregates, the balance being ground beef meat as bought in thestore, and it was found that all of the patties so prepared, bycomparison with controls, had the familiar hamburger fiavor and werequite palatable. With respect to mouth feel, none gave any indication ofthe presence of the aggregates. Of additional interest were the findingsthat the aggregatescontaining patties underwent less shrinkage than thecontrols, had much less tendency to burn, and had an interestingvariation in respect of their chewiness.

Another contemplated application of the invention is in dairy productfoods such as cheese and in foods using milk and cream. N t .rally softand semi-soft non-gratable cheeses may, by mixing the same with theaggro gates, be transformed into a dry granular free-flowing form,making it more convenient to handle such cheeses when they are used asingredients in a recipe. Milk and cream may be used more convenientlywhen mixed with the aggregates. For example, cream as obtained frommilk, either with or without the preliminary removal of Water from thecream, may be mixed with the aggregates to form a dry free-flowingmixture for use, say, in coffee, and if desired, the mixture may bepackaged in inexpensive, single use, disposable paper containers,although it may also be stored in bulk and dispensed in any desired way,that is, by machine or by hand. In the result, there is provided a lowcalorie cream-containing mix whose use with coffee and other substancessimulates natural cream.

The aggregates are also suitable for use in confections, includingcandy, chewing gum, bakers confections, etc. Particularly in candy, theaggregates have a tendency to decrease or cut the sweet taste to anextent, especially in candy of pronounced sweetness, without resortingto synthet c or substitute sweetening agents. Edible food dyes may beincorporated in the candy in a convenient mannor by first sorbing a dyeon and in the aggregates and then mixing in the latter with the othercandy ingredients. In chewing gum the aggregates are of value forintroducing flavors. Thus, a flavor-containing substance may be formedinto a granular free-flowing miX with the aggregates, and the resultingmixture may be incorporated with the chicle or other chewable plasticgum. base. Blooming of chocolate and other foods, comprsing the releaseof oil, may be lessened through use of the aggregates.

Vegetables, fruits, and nuts may be benefited by the aggregates. Forexample, part of the vegetables used in soup bases may be replaced bythe aggregates to eifect a calorie reduction; or a color lighteningeffect, or a thickening of the soup may be achieved with or withoutreplacing conventional ingredients. Shelled nuts may be thinly coatedwith powdered aggregates to improve their storage life. Miscellaneousfoods in which the crystallite aggregates may be incorporated toadvantage are gravies, sauces, jellies, jams, preserves, molasses,beverages, and the like. The aggregates provide a th ckening effect insuch foods as sauces and gravies.

With respect to their general application in foods, the aggregates mayserve to replace, in whole or part, one or more components of a givenfood, particularly high calorie components such as fats and oils, sugar,and starch. Or they may replace conventional binders in many foods. Inother instances they may simply be added to a conventional recipe todecrease the over-all calorie value, it being understood that the amountof the remaining components of the recipe will be proportionatelydecreased. In addition to the reduction in calories, and the variousSalt other benefits described, the employment of the aggregates bringsabout still another and substantial result by virtue of theirtherapeutic value as a safe, wholesome laxative.

In other instances the aggregates, by virtue of their compressibility,help to provide food products that may be shaped by compression into anysuitable form, using compression pressures of up to 5000 psi. or more.Many of the aggregates-containing food mixtures, such as thoseillustrated in Examples 10, 14 and 19 below, are also extrudable,particularly those wherein the food contains one or more liquidingredients. Lightening of the color of a food product is possible byuse of the aggregates, some fractions of which, as described, arecharacterized by being intensely white and opaque. As also described,dry mix foods of the convenience and instant types are easily prepared,even from liquid-containing ingredients, because of the unusually goodsorptivc action of the aggregates on liquids. The cuttability of manyfood products is improved by the aggregates, and they further tend toretard the melting, in warm climates, of meltable components.

The aggregates have no adverse effect on the food or food ingredientswith which they are mixed; and similarly are not themselves adverselyaffected. in some cases they exert a protective or preservative action;thus, in one instance a 64:36 parts by Weight mixture of blue cheese andthe aggregates showed no noticeable change in appearance, consistency,aroma, or taste after being kept in a stoppered glass container for 5months at room temperature.

The amount of aggregates incorporated in a food composition is variable,depending on the particular food, on whether or not an ingredient oringredients is being replaced in whole or part, on the mouth textureand/or body desired, etc. The amount may vary from a concentration aslow as about 6.1%, or less, to or more, bye weight; but usually theamount is from about 5% to 25% by weight, and more preferably from about5 to 20% by weight. i

In some cases it is desirable to incorporate with the crystalliteaggregates a small amount of a protective colloid to vary the texture ormouth feel of the resulting mix or food product, it being possible toincrease the smoothness, or impart some chewiness, etc. The amount ofsuch colloid may range from a tenth to a few percent, say from 0.1 toabout 5%, preferably 0.1 to 2 or 3% by weight of the food product, andthe colloid may be chosen from conventional materials such for instanceas carrageenin, tragacanth, arabic, ghatti, and karaya gums; seaweedcolloids such as agar, carrageen and sodium alginate; seed extracts suchas locust bean, quince and guar; starches and starch derivatives, likeconverted starches; waterdispersible cellulose derivatives such assodium cal-boxymethylcellulose; pectins such as apple pectin and citruspectin; and modified pectins such as low methoxy pectins. Fropyleneglycol alginate, glycerol, and stearic acid monoand diglycerides arealso useful.

The invention may be illustrated by the following examples.

Example 1 Honey-flavored doughnuts were prepared having the followingcomposition:

Ingredient Gms. /batch Perctnt Eggs, fresh Sugar Grystallite agShortening. Baking pow Cinnamon. Nutmeg... Baking soda. Flour 11 Thecrystallite aggregates were prepared by hydrolyzing Ketchikan wood pulpwith a 0.5% HCl solution for 60 minutes at 250 F. The aggregates werewashed with water and then dried in an oven at 65 C. for 24 hours undera vacuum of 29 inches of water. They had an average level-oft D.P. of220, a moisture content of 2.5% by weight, and a particle size in therange of l to 300 microns. The dried aggregates were first mixed withthe honey by placing the latter in the bowl of a Model N-5 variablespeed Hobart mixer equipped with a paddle or beater attachment and themixer set in operation at a low speed corresponding to about 61 rpm. Thebeater comprised a stem having a plurality of spaced arms ex tendingangularly downwardly from opposite sides, and a substantially V-shapedmember connected the outer ends of the arms; in effect, the paddleresembled an inverted tree. The beater rotated and revolved in the bowl.In other words, it had a compound action: it revolved inside the bowl,and it rotated on its axis, the direction of rotation being opposite thedirection of its 4 movement around the bowl. The addition of the finelydivided aggregates was done over a period of about 5 to minutes, themixture being converted to a freely flowable dry mass which was removedfrom the Hobart. The eggs were then beaten in the Hobart, and to themwere added, during agitation, the sugar, and the aggregateshoney drymass. The milk and the melted shortening (hydrogenated vegetable oil)were next added to the mix. Then the baking powder (monocalciurnphosphate), salt, cinnamon, nutmeg, and baking soda (sodium bicarbonate)were combined and added, with agitation. Finally, the flour was addedand mixing continued to form a smooth dough. The latter was chilled in arefrigerator, the dong nuts then formed therefrom and deep fat fried atabout 370 F. They appeared to be normal in every observable respect,including their eating quality, by comparison with control doughnutsmade at the same time wherein the aggregates were omitted. A secondbatch was made in which the aggregates content was only 5%, and thesealso were indistinguishable from the conventional doughnuts. As a resultof the frying process, the doughnuts containing 5% aggregates showed aweight gain of 9.68%, while those containing 12.6% aggregates gained2.45%. Satisfactory doughnuts were also made containing up to by weightof the aggregates.

Example 2 A peanut butter cookie dry mix was prepared from the followingingredients:

The crystallite aggregates were prepared as in Example 1. The peanutbutter and the butter mere first mixed with the dried aggregates in theHobart mixer to form a free flowing dry mass, after which all of theremaining ingredients were added, with mixing. Then there were added tothe mix in the Hobart, with continued agitation, /2 teaspoon vanilla,one egg, and 185 m1. of water. The resulting heavy dough was rolled intosmall balls, flattened with a fork on a greased coolde sheet, and bakedfor 15 minutes in an oven preheated to 375 F. The flavor and eatingquality of the resulting cookies were particularly excellent, and inother respects they were equal to the conventional product.

Example 3 Cellulose crystallite aggregates were prepared by hydrolyzingKetchikan wood pulp with 2.5 normal HCl solution for 15 minutes atboiling temperature. The aggregates were washed with water and thendried at 65 C. They had an average level-oil D1. of 220, a moisturecontent of about 5% by weight, and a particle size in the range of 1 to300 microns. Then a cup of wheat bran and cup of milk were mixedtogether and allowed to stand until the bran had absorbed the maximumamount of moisture. The cup used had a liquid capacity of about 250 ml.when full. One egg and A cup of shortening were mixed with the moistenedbran and the mixture was beaten well. Then a cup of the dried aggregateswas stirred with the bran mixture, and 2 /2 tsp. baking powder, tsp.salt, and A cup sugar were also stirred into the mixture. Greased mutlinpans were filled 'full with the resulting doughy mixture and the latterbaked in a moderately hot oven of about 400 F. for 30 minutes. Theresulting bran mufiins had the texture of conventional bran muffins, butthe crumb was lighter in color; they were easily broken and easilychewed, and had an aggregates content of about 18% by weight.

Example 4 A layer cake was prepared as follows. One cup of sugar and /2cup butter were blended together and mixed with 3 well beaten eggs. Acup of pastry flour and a cup of dried powdered cellulose crystalliteaggregates were mixed together, the latter prepared as in Example 3.Then 3 tsp. of baking powder were added to the flouraggregates mixtureand the latter sifted three times. Portions of the flour mixture wereadded to the sugar-butteregg mixture, alternating with small additionsof milk, until all of the flour mixture and /3 cup of milk were added. Atsp. of vanilla was added and the mix was well beaten. It was baked inan oven for 25 minutes at 375 F. and resulted in a white-colored, lowSugar layer cake of very good texture and containing about 13% by weightof the aggregates. The cake was finished off by applying to it achocolate topping as prepared in Example 7.

Example 5 Dried cellulose crystallite aggregates, of the kind used inthe preceding example, were mixed with cornstarch to form a powderedmixture comprising dried aggregates and 10% cornstarch. The mixture waswetted with water to form a thick extrudable paste, and this was thenextruded through a stainless steel tube having a single opening of 34inch diameter at its discharge end. The mixture extruded smoothly,forming monofils of more or less continuous lengths, which were thendried in an oven at about 60 C., to produce hard spaghetti-like strands.These were broken to V2 to 1 inch lengths. When tasted, the driedproduct was crisp, fairly hard, and edible. A like product, butcontaining a chocolate flavoring material, had better palatability. Bothproducts had good chewiness, and were considered to be suitable as afibrous breakfast food, or as a basis therefor, particularly whenmodified by the addition of other ingredients, such as a flavor,sweetening agent, other cereal grain, and the like. Soft-texturedproducts are obtained by decreasing the amount of aggregates in theextrudable mixture, although at an aggregateswornstarch ratio of 50:50the product had a somewhat gummy mouth feel.

Example 6 Never dried cellulose crystallite aggregates, prepared byhydrolyzing Ketchikan wood pulp with 2.5 normal I-ICl solution at theboil for 15 minutes, and having an average level-off DP. of 220, amoisture content of 64%, and a particle size in the range of 1 to 300microns, were diluted with water to a solids content of 30% andsubjected to attrition in a Waring Blendor for a period of 15 minutes,there being formed a stable homogeneous colloidal gel having 30% solids.Then a square of unsweetened chocolate was melted and mixed with /2. cup

of sugar, /s tsp. of salt, and 2 cups of milk. The resulting mixture washeated, with stirring, until uniform, after which the above describedgel was stirred in until a pudding-like consistency was reached. Thelatter mixture was chilled in a deep freezer and then removed. Itcomprised a chocolate pudding of smooth texture, somewhat firmconsistency, and having the appearance of a conventional pudding. It hada good chocolate flavor and better than average palatability. Theaggregates content was about 15% by weight.

Example 7 A portion of the chocolate pudding of Example 6 was dilutedwith a 10% aggregates-containing gel, the latter being formed bydiluting the 30% gel of the preceding example, and the mixture wasthoroughly stirred while heating for about 4 minutes. Upon cooling toroom temperature, a smooth creamy chocolate sauce or dessert topping wasobtained. The product had the consistency of heavy syrup, was suitablyflowable, and had the color of milk chocolate. Its eating quality wasvery good, with no evidence of the presence of the aggregates.

Example 8 A half-cup of sugar and -6 drops of vanilla were thoroughlymixed in a Waring Blender with 2 cups of a stable aqueous colloidal gelcontaining 20% by weight of crystallite aggregates prepared as inExample 6. The mixture was then chilled, giving an attractive-looking,snow white, vanilla-flavored, smooth-textured puddIng which had theconsistency of soft ice cream. It had about 16% by weight of aggregates.

Example 9 Never dried cellulose crystallite aggregates, prepared byhydrolyzing Ketchikan wood pulp with 0.64% HCl solution at 250 F. forhour, and having an average level-off D.P. of 220 and a moisture contentof 66%, were diluted with water to a solids content of 13% and then, inan amount of 39 gms., were subjected to attrition in the Waring Blendorfor 6 minutes together with 30 gms. of sugar, 229.8 gms. water, 0.3 gm.vanilla, and 0.9 gm. of sodium alginate. The weight percentagecomposition of the resulting smooth gel pudding was aggregates 13%,sugar vanilla 0.1%, alginate 0.3%, and water 76.6%. The pudding had asmooth texture and an over-all palatable taste. It had a calorie valueof about 0.4 calorie per gram, as compared with about 0.9 calorie pergram for a conventional pudding wherein.

cornstarch is present in place of the aggregates. The pudding did notappear to be affected by increasing the aggregates content to by weight.Suitable puddings were also prepared omitting the alginate.

Example 10 Ingredient (Ems/batch Percent Peanut butter 45. 0 29. 0 Brownsugar 75.0 48. 2 Crystallite aggregates".-- 35.0 22. 8

.1 Example 11 A reduced calorie cream salad dressing was prepared havingthe following composition:

Ingredient Gms'Jbateli Percent Calories Crystallite aggregates 143. 815. 56 Total water 426. 3 46. 13 68. 0 7. 36 29. 2'8 14. 4 1. 56 1. 6 17.37 1 01 04 4 .04 30. 0 3. 25 12. 92 80. 0 8. 66 77. 92 16. O 1. 73 6.15 121.0 13.09 1. 57 20. 0 2. 16 87 2. 5 27 38 The crystalliteaggregates were prepared as in Example 1, except that they were notdried, the moisture content being about 65%. The never dried aggregates,at a consistency of about 33% solids, were attrited for 20 minutes inthe Hobart mixer at an intermediate speed of about 125 rpm. to produce asmooth gel. Then the sugar, salt, mustard, glutamate, and celery saltwere premixed and added to the aggregates in the Hobart, with mixing,followed by the addition of the glycerol, cottonseed oil, egg yolk,vinegar and lemon juice, in that order. After further mixing, the sodiumalginate was dissolved in water and added to the mix, and agitation wascontinued until the batch was smooth.

From a flavor standpoint, the product compared favorably withconventional salad dressing and mayonnaise. When stored for 3 months at40 F. in a household refrigerator, the product showed no signs ofviscosity loss or free water accumulation. The calorie values of theingredients of the product, which appear in the table above, were takenfrom Nutritional Data Handbook published by H. J. Heinz Co. and refer tothe weight percent composition of the dressing, rather than the gramsper batch basis. In other words, if the weight percent values areconsidered to be on a gram basis, then the listed calorie values areapplicable; for example, grams of the dressing have a nutritive value of129.5 calories. On a per gram basis, the calorie content of the productis 1.30 calories. Conventional cream salad dressing has a value of 3.90cal./gm., and mayonnaise a value of 7.20 cal./ gm. Further reduction ofthe calorie content of the product is possible, without any appreciableloss of quality and eifectiveness, by reducing the amount of the cottonseed oil to 50% or less of its present concentration.

Example 12 A 30% gel of crystallite aggregates was prepared, as inExample 6, and to a 500 ml. volume of the gel there were added tsp. ofsalt, /2 cup of corn oil, and 3 gms. of CMC (sodiumcarboxymethylcellulose) as an emulsifier. These ingredients were mixedin the Waring Blendor until a creamy butterlike product resulted thathad the appearance of butter or oleomargarine. The product waspalatable, having a flavor similar to butter, and was soft and easilyspread. There was no visible oiling 011. The material, which containedabout 24% by weight of the aggregates and had a calorie value only afraction of that of butter or margarine, was considered suitable as areplacement for either of the latter.

Example 13 A mayonnaise type salad dressing was prepared by thoroughlymixing /2 cup of corn oil, 1 tsp. of vinegar, and /8 tsp. of salt with 1cup of a stable aqueous 15% colloidal gel of cellulose crystalliteaggregates, prepared as in Example 6. The mixture was churned in theWaring Blendor for about 5 minutes, at the end of which 15 time a smoothstable yellowish-looking salad dressing was obtained which had a texturelike that of whipped cream and which very much resembled conventionalmayonnaise in flavor, appearance, and consistency. It contained about20% by weight of the aggregates.

Example 14 A conventional meat emulsion for making frankfurters wasobtained from a commercial source, it having been made up in aconventional Way. It comprised boneless chucks, pork trimmings, spices,seasonings, salt, sugar, and curing salts and was in the form of amoist, brownish, plastic, cohesive, tacky mass. While still in a chilledstate, the mass was divided into portions and handled as follows:

(1) A ZOO-gm. portion was taken as a control and stuffed into a 2-inchdiameter regenerated cellulose sausage casing. This step was donemanually to observe at first hand the flow characteristics of theemulsion, which were considered to be difficult at best owing to thetackiness.

Occlusion of air bubbles was a problem. The ends of the stutled casingwere tied to form a brownish-colored sausage link.

(2) A mixture of 95 gms. of the emulsion and gms. of crystalliteaggregates was prepared in the Hobart mixer. The resulting 5%aggregates-containing mixture was substantially indistinguishable fromthe control although it was thought that the mixture had acquired somefirmness. The mixture was packed with difiiculty into a length ofsausage casing. The color of the link was substantially the same as thecontrol link. The aggregates, which were prepared by hydrolyzingKetchikan wood pulp with 0.5% HCl solution at 250 F. for 1 hour, had aD1. or" 220 and were dried to a moisture content of 2.5%.

(3) Using the crystallite aggregates described, a aggregates-containingmixture, comprising 90 gms. of meat emulsion and 10 gms. of aggregates,was prepared in the Hobart, and while the resulting mass was stillplastic and cohesive, some loss of tackiness was noticeable. The mixturewas more easily packed into the casing, and the resulting link hadsubstantially the same color as the control.

(4) A aggregates mixture was prepared from 160 gms. of emulsion and gms.of aggregates, there being produced a cohesive dough which was much lesstacky and sticky than the control mass and which appeared to haveextrudable properties. The mixture was much easier to stuff into thecasing, and the resulting link, while still generally resembling thecontrol link, was noticeably lighter in color than the latter.

All of the links were then heated for about 1% rs. at 160 F., at the endof which time it was noticed that some oily amber fluid had colected ineach link just beneath the casing, there being less fluid in the case ofthe N0. 4 than the others. The control and Nos. 2 and 3 were red incolor, no diiferences being apparent in this respect, While No. 4 wasslightly less red than the others. The control link was softer to thetouch than the others.

All links were immediately transferred to water maintained at 160 F. andwere allowed to cook therein for 12 minutes. The control and Nos. 2 and3 remained red in color during the cooking while No. 4 first appeared toacquire a brownish hue and then became pink. The links were next placedunder a shower of cold tap water for 5 minutes and then were storedovernight in a refrigerator at F.

Upon examination, all the links had the same general red color exceptthat No. 4 was more pink than red. All had oily liquid disposed justbeneath the casing, No. 4 having less than the others. No shrinkage wasapparent, although in No. 4 the meat mixture filled the casing betterthan in the other links. The control was sott-to-firm to the touch, andthe others were firmer, the degree of firmness increasing with theconcentration of aggregates. All links were easily cut. A comparison ofthe cut surfaces AK? showed that Nos. 2 and 3 appeared meatier" than thecontrol, that is, the cut surfaces of Nos. 2 and 3 appeared to have atruer, more fibrous meat texture. No. 4 also looked meatier than thecontrol but less than Nos. 2 and 3. None of the links crumbled oncutting, and all had the normal aroma of cooked frankfurters. Cut slicesof Nos. 2 and 3 were spreadable, the latter to a greater degree, whereasthe control and No. 1 would not spread, appearing somewhat rubbery inthis respect.

Tasting and eating of the links by a panel showed the following: theflavor of the control, Nos. 2 and 3 was considered superior to that ofstore-bought frankfurters, while that of No. 4 was considerably lessthan the others. The control had a soft chewy texture and an excellenteating quality, while Nos. 2 and 3 were each slightly more chewy and hadexcellent eating quality. No. 4 was thought to have less chewiness thanthe others in that it was less cohesive in the mouth. The control wasvery juicy but was exceeded in this respect by No. 2, while No. 3 wasabout equal to the control. No. 4 had some juiciness. Over-all, thecontrol and Nos. 2 and 3 were judged very palatable and No. 4 less so.

Example 15 About 200 grams of Cheddar cheese were mixed in the Hobartmixer with crystallite aggregates of the kind used in Example 1, exceptthat they had been dried to a moisture content of about 4%. Theaggregates were added slowly, with agitation. When the aggregates-cheesemixture was in approximately a 1:4 weight ratio, a dry freefiowingmixture was obtained having an average particle diameter of about onemillimeter. By mixing 6 parts of the dry cheese mixture and 4 parts ofwater, a reduced calorie product similar to a cheese spread was obtainedhaving a homogeneous all-cheese mouth feel. The spread contained about18% by weight of the aggregates.

Example 16 A dry mix ice cream was prepared as follows: driedcrystallite aggregates and coconut oil were mixed in the Hobart to forma finely divided free-flowing crumb comprising 52% aggregates and 48%oil. The aggregates were prepared as in Example 1. Then 83.2 gms. of thecrumb were dry-mixed in the Hobart with 60 gms. sugar, 48 gms. of drymilk-solids-not-fat, and 0.8 gm. of sodium alginate to produce a finefree-flowing dry ice cream mix. This mixture was then beaten with 208ml. of water in a Mixmaster mixing device until thoroughly dispersed,placed in an ice cube tray, and stored in the freezer compartment of ahousehold refrigerator for 1 hour. The resulting ice cream product hadthe taste and texture of conventional ice cream and was considered to bepalatable. It had better resistance to melt down than the conventionalproduct. The weight percentage composition was: fat 10%, sugar 15%,milk-solids-not-fat 12%, alginate 0.2%, crystallite aggregates 10.8%,and water 52%.

Example 17 One cup of the chocolate pudding of Example 6 was stirredinto 2 cups of milk and malt flavor was added. The mixture was thenwhipped in a Waring Blendor for about 5 minutes, there being formed asmooth creamy liquid closely resembling a malted milk shake inappearance, body, and texture. It had an excellent flavor, a consistencyof light cream, and was considered very palatable. The aggregate contentwas about 5% by weight.

Example 18 A cup of commercial catsup was mixed with 3 cups of water andheated to the boil, producing a very fluid mixture; then 2 cups of asmooth stable aqueous colloidal gel containing 20% by weight ofcellulose crystallite aggregates and prepared as in Example 6, werethoroughly stirred into the heated mixture, there being formed a smoothcreamy product. After cooling, the mixture became quite thick. Theaggregates had a lightening or whitening as well as a thickening effecton the tomato catsup, and the product had the appearance, texture, body,and flavor of a conventional creamed tomato soup. The aggregatesconcentration was about 7%.

Example 19 A batch of caramel candy was made up and divided into 4parts, the first being a control, while the second, third, and fourthparts were the same except that they additionally contained,respectively, 5, 10, and 14.4% of crystallite aggregates. Thecompositions of these batches in grams were as follows:

The crystallite aggregates were prepared by hydrolyzing Ketchikan woodpulp with 0.5% HCl solution at 250 F. for hour. They had an averagelevel-off DR of 240 and were dried to a moisture content of about 2%.Water was present in each composition as the evaporated whole milkcomprised about 72% by weight of water, the corn syrup had an averagewater content of 19%, and the butter about 15.5%; thus, the controlsample, for example, contained about 20% by weight of water. The candywas prepared conventionally, the corn syrup, sugar, and salt being firstslowly cooked together, followed by the addition of the butter. Then themilk was added drop by drop, and cooking continued slowly to atemperature of about 238 F after which the chocolate was added. Thematerial was transferred to buttered pans and cooled. In Nos. 2 and 3,the crystallite aggregates were added to the batch after the addition ofthe butter, and in No. 4 the aggregates addition was made following themilk.

All samples had a normal appearance, and this was also true of cutsurfaces of the control and Nos. 1 and 2. The cut surface of No. 3lacked the smooth look of caramel, appearing to have a somewhat coarsetexture. All samples had a dark brown color. The flavor of the controland Nos. 1 and 2 was very good, while No. 3 was considered to be good.The control and No. 1 had a typically smooth caramel texture and chewyquality; No. 2 was slightly drier and slightly less cohesive in themouth and appeared to resemble Toosie-Roll candy. No. 3 had a fudge-liketexture and was less cohesive than No. 2, however, it was judged to bepalatable although not to the same extent as the control and Nos. 1 and2. Generally, as the crystallite aggregates content increased, the candyappeared to become less sweet to the taste and less cohesive in respectof its mouth feel.

Example 20 A quantity of conventional milk chocolate was melted, addedto the Hobart mixer, and then followed by the addition of a sufficientamount of dried crystallite aggregates to produce a dry, free-flowingpowder containing about 32% by weight of the aggregates. The latter wereprepared as in Example 1 except that the moisture content was about 5%by weight. Then 6 parts of water were added to 4 parts of the powder,with stirring, to form an instant spread which had all of the flavor,aroma and taste of the original chocolate. The spread contained about13% by weight of the aggregates.

In all of the products described in the examples, unless notedotherwise, the presence of the crystallite aggregates was not detectableby the mouth feel of the products.

Although the invention has been described in connection with specificembodiments of the same, it will be understood that it is capable ofobvious variations without departing from its scope.

In the light of the foregoing description, the following is claimed:

1. A reduced calorie food composition comprising a mixture of a foodmaterial and cellulose crystallite aggregates; said aggregates per -secomprising the acid-insoluble crystalline residue of the acid hydrolysisof cellulose and being characterized by the uniformity of the lengths ofthe constituent chains thereof, said aggregates having an averagelevel-01f D.P. of 15 to 375 anhydroglucose units, the constituent chainsof each aggregate being separate from and free of those in neighboringaggregates, said aggregates being further characterized by having asharp X-ray dilfraotion pattern indicative of a substantiallycrystalline structure, and said aggregates having a bland taste and odorand being edible but not nutritious; said composition having the eatingquality of the food material.

2. A reduced calorie food composition incorporating therein, as anon-nutritive substance, mechanically disintegrated cellulosecrystallite aggregates, said aggregates comprising the acid-insolublecrystalline residue of the acid hydrolysis of cellulose and beingcharacterized by the uniformity of the lengths of the constituent chainsthereof, said aggregates having an average level-off D.P. of 15 to 375anhydroglucose units, the constituent chains of each aggregate beingseparate from and free of those in neighboring aggregates, saidaggregates being further characterized by having a sharp X-raydilfraction pattern indicative of a substantially crystalline structure,by having a chemical purity of at least an ash content of less than 600p.p.m., and a particle size in the range of less than 1 to 300 microns,and said aggregates comprising straight, rigid, relatively non-twistablegroups of linear chains.

3. The product of claim 1 in which at least 1% by weight of thecellulose crystallite aggregates in the composition having a particlesize of up to 1 micron.

4. A reduced calorie bakery food composition of claim 1 in which thefood material includes a bakery ingredient.

5. A reduced calorie oleaginous food composition of claim 1 in which thefood material includes an edible oleaginous material.

6. A reduced calorie aqueous food composition of claim 1 in which thefood material includes an edible aqueous liquid and at least 1% byweight of said cellulose crystallite aggregates have a particle size upto 1 micron.

7. The reduced calorie aqueous food composition of claim 6, which foodcomposition is in the liquid state.

8. The reduced calorie aqueous food composition of claim 6, whichcomposition is in the frozen state.

References Cited in the file of this patent UNITED STATES PATENTSWallach Nov. 17, 1942 OTHER REFERENCES

1. A REDUCED CALORIE FOOD COMPOSITION COMPRISING A MIXTURE OF A FOODMATERIAL AND CELLULOSE CRYSTALLITE AGGREGATES; SAID AGGREGATES PER SECOMPRISING THE ACID-INSOLUBLE CRYSTALLINE RESIDUE OF THE ACID HYDROLYSISOF CELLULOSE AND BEING CHARACTERIZED BY THE UNIFORMITY OF THE LENGTHS OFTHE CONSTITUENT CHAINS THEREOF, SAID AGGREGATES HAVING AN AVERAGELEVEL-OFF D.P. OF 15 TO 375 ANHYDROGLUCOSE UNITS, THE CONSTITUENT CHAINSOF EACH AGGREGATE BEING SEPARATE FROM AND FREE OF THOSE IN NEIGHBORINGAGGREGATES, SAID AGGREGATES BEING FURTHER CHARACTERIZED BY HAVING ASHARP X-RAY DIFFRACTION PATTERN INDICATIVE OF A SUBSTANTIALLYCRYSTALLINE STRUCTURE, AND SAID AGGREGATES HAVING A BLAND TASTE AND ODORAND BEING EDIBLE BUT NOT NUTRITIOUS; SAID COMPOSITION HAVING THE EATINGQUALITY OF THE FOOD MATERIAL.